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An electron cyclotron resonance (ECR) ion source (ECRIS) can generate an available amount of multicharged ions, thus it is not limited for use in the field of accelerator science, but also in medical/biological fields, such as for heavy ion beam cancer treatment and ion engines. The processes of generating multicharged ions are mainly sequential collisions of a direct ionization process by electrons, and have good ion confinement characteristics. By utilizing this confinement property, we have synthesized iron-encapsulated fullerenes, which are supramolecular and can be expected to have various high functions. Fullerenes and iron ions are vaporized from pure solid materials and introduced into the ECRIS together with the support gas. We investigated conditions under which fullerene ions do not dissociate and iron ions are generated so that both can coexist. Generated ions are extracted from the ECRIS and separated by mass/charge with a dipole magnet, and detected with a Faraday cup. This measurement system is characterized by a wide dynamic range. The charge-state distribution (CSD) of ion currents was measured to investigate the optimum conditions for supramolecular synthesis. As a result, a significant spectrum suggesting the possibility of iron-encapsulated fullerenes was obtained. This paper describes the details of these experimental results.